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Sulfur trioxide (SO3) is an important oxide of sulfur and a key intermediate in the formation of sulfuric acid (H2SO4, SA) in the Earth's atmosphere. This conversion to SA occurs rapidly due to the reaction of SO3 with a water dimer. However, gas-phase SO3 has been measured directly at concentrations that are comparable to that of SA under polluted mega-city conditions, indicating gaps in our current understanding of the sources and fates of SO3. Its reaction with atmospheric acids could be one such fate that can have significant implications for atmospheric chemistry. In the present investigation, laboratory experiments were conducted in a flow reactor to generate a range of previously uncharacterized condensable sulfur-containing reaction products by reacting SO3 with a set of atmospherically relevant inorganic and organic acids at room temperature and atmospheric pressure. Specifically, key inorganic acids known to be responsible for most ambient new particle formation events, iodic acid (HIO3, IA) and SA, are observed to react promptly with SO3 to form iodic sulfuric anhydride (IO3SO3H, ISA) and disulfuric acid (H2S2O7, DSA). Carboxylic sulfuric anhydrides (CSAs) were observed to form by the reaction of SO3 with C2 and C3 monocarboxylic (acetic and propanoic acid) and dicarboxylic (oxalic and malonic acid)-carboxylic acids. The formed products were detected by a nitrate-ion-based chemical ionization atmospheric pressure interface time-of-flight mass spectrometer (NO3--CI-APi-TOF; NO3--CIMS). Quantum chemical methods were used to compute the relevant SO3 reaction rate coefficients, probe the reaction mechanisms, and model the ionization chemistry inherent in the detection of the products by NO3--CIMS. Additionally, we use NO3--CIMS ambient data to report that significant concentrations of SO3 and its acid anhydride reaction products are present under polluted, marine and polar, and volcanic plume conditions. Considering that these regions are rich in the acid precursors studied here, the reported reactions need to be accounted for in the modeling of atmospheric new particle formation.
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New particle formation (NPF) is a major source of atmospheric aerosol particles, including cloud condensation nuclei (CCN), by number globally. Previous research has highlighted that NPF is less frequent but more intense at roadsides compared to urban background. Here, we closely examine NPF at both background and roadside sites in urban Central Europe. We show that the concentration of oxygenated organic molecules (OOMs) is greater at the roadside, and the condensation of OOMs along with sulfuric acid onto new particles is sufficient to explain the growth at both sites. We identify a hitherto unreported traffic-related OOM source contributing 29% and 16% to total OOMs at the roadside and background, respectively. Critically, this hitherto undiscovered OOM source is an essential component of urban NPF. Without their contribution to growth rates and the subsequent enhancements to particle survival, the number of >50 nm particles produced by NPF would be reduced by a factor of 21 at the roadside site. Reductions to hydrocarbon emissions from road traffic may thereby reduce particle numbers and CCN counts.
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Material Particulado , Emisiones de Vehículos , Contaminantes Atmosféricos , Monitoreo del Ambiente , Tamaño de la Partícula , AerosolesRESUMEN
Although many studies have discussed the impact of Europe's air quality, very limited research focused on the detailed phenomenology of ambient trace elements (TEs) in PM10 in urban atmosphere. This study compiled long-term (2013-2022) measurements of speciation of ambient urban PM10 from 55 sites of 7 countries (Switzerland, Spain, France, Greece, Italy, Portugal, UK), aiming to elucidate the phenomenology of 20 TEs in PM10 in urban Europe. The monitoring sites comprised urban background (UB, n = 26), traffic (TR, n = 10), industrial (IN, n = 5), suburban background (SUB, n = 7), and rural background (RB, n = 7) types. The sampling campaigns were conducted using standardized protocols to ensure data comparability. In each country, PM10 samples were collected over a fixed period using high-volume air samplers. The analysis encompassed the spatio-temporal distribution of TEs, and relationships between TEs at each site. Results indicated an annual average for the sum of 20 TEs of 90 ± 65 ng/m3, with TR and IN sites exhibiting the highest concentrations (130 ± 66 and 131 ± 80 ng/m3, respectively). Seasonal variability in TEs concentrations, influenced by emission sources and meteorology, revealed significant differences (p < 0.05) across all monitoring sites. Estimation of TE concentrations highlighted distinct ratios between non-carcinogenic and carcinogenic metals, with Zn (40 ± 49 ng/m3), Ti (21 ± 29 ng/m3), and Cu (23 ± 35 ng/m3) dominating non-carcinogenic TEs, while Cr (5 ± 7 ng/m3), and Ni (2 ± 6 ng/m3) were prominent among carcinogenic ones. Correlations between TEs across diverse locations and seasons varied, in agreement with differences in emission sources and meteorological conditions. This study provides valuable insights into TEs in pan-European urban atmosphere, contributing to a comprehensive dataset for future environmental protection policies.
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Contaminantes Atmosféricos , Ciudades , Monitoreo del Ambiente , Material Particulado , Oligoelementos , Material Particulado/análisis , Contaminantes Atmosféricos/análisis , Oligoelementos/análisis , Monitoreo del Ambiente/métodos , Europa (Continente) , Atmósfera/química , Estaciones del Año , Contaminación del Aire/análisisRESUMEN
Although leaded gasoline was banned at the end of the last century, lead (Pb) remains significantly enriched in airborne particles in large cities. The remobilization of historical Pb deposited in soils from atmospheric removal has been suggested as an important source providing evidence for the hypothetical long-term persistency of lead, and possibly other pollutants, in the urban environment. Here, we present data on Pb isotopic composition in airborne particles collected in London (2014 to 2018), which provide strong support that lead deposited via gasoline combustion still contributes significantly to the lead burden in present-day London. Lead concentration and isotopic signature of airborne particles collected at a heavily trafficked site did not vary significantly over the last decade, suggesting that sources remained unchanged. Lead isotopic composition of airborne particles matches that of road dust and topsoils and can only be explained with a significant contribution (estimate of 32 ± 10 to 43 ± 9% based on a binary mixing model) of Pb from leaded gasoline. The lead isotopes furthermore suggest significant contributions from nonexhaust traffic emissions, even though isotopic signatures of anthropogenic sources are increasingly overlapping. Lead isotopic composition of airborne particles collected at building height shows a similar signature to that collected at street level, suggesting effective mixing of lead within the urban street canyon. Our results have important implications on the persistence of Pb in urban environments and suggest that atmospheric Pb reached a baseline in London that is difficult to decrease further with present policy measures.
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Atmósfera/química , Plomo/análisis , Contaminantes Atmosféricos/análisis , Monitoreo del Ambiente , Gasolina/análisis , Historia del Siglo XX , Isótopos/análisis , Londres , Material Particulado/análisis , Factores de TiempoRESUMEN
New particle formation (NPF) is a leading source of particulate matter by number and a contributor to particle mass during haze events. Reductions in emissions of air pollutants, many of which are NPF precursors, are expected in the move toward carbon neutrality or net-zero. Expected changes to pollutant emissions are used to investigate future changes to NPF processes, in comparison to a simulation of current conditions. The projected changes to SO2 emissions are key in changing future NPF number, with different scenarios producing either a doubling or near total reduction in sulfuric acid-amine particle formation rates. Particle growth rates are projected to change little in all but the strictest emission control scenarios. These changes will reduce the particle mass arising by NPF substantially, thus showing a further cobenefit of net-zero policies. Major uncertainties remain in future NPF including the volatility of oxygenated organic molecules resulting from changes to NOx and amine emissions.
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Contaminantes Atmosféricos , Contaminación del Aire , Beijing , Tamaño de la Partícula , Monitoreo del Ambiente/métodos , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Material Particulado/análisis , Aminas , Contaminación del Aire/prevención & control , Contaminación del Aire/análisisRESUMEN
Biomass burning is common in much of the world, and in some areas, residential wood-burning has increased. However, air pollution resulting from biomass burning is an important public health problem. A sampling campaign was carried out between May 2017 and July 2018 in over 64 sites in four sessions, to develop a spatio-temporal land use regression (LUR) model for fine particulate matter (PM) and wood-burning tracers levoglucosan and soluble potassium (Ksol) in a city heavily impacted by wood-burning. The mean (sd) was 46.5 (37.4) µg m-3 for PM2.5, 0.607 (0.538) µg m-3 for levoglucosan, and 0.635 (0.489) µg m-3 for Ksol. LUR models for PM2.5, levoglucosan, and Ksol had a satisfactory performance (LOSOCV R2), explaining 88.8%, 87.4%, and 87.3% of the total variance, respectively. All models included sociodemographic predictors consistent with the pattern of use of wood-burning in homes. The models were applied to predict concentrations surfaces and to estimate exposures for an epidemiological study.
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Contaminantes Atmosféricos , Material Particulado , Material Particulado/análisis , Contaminantes Atmosféricos/análisis , Madera/química , Chile , Monitoreo del Ambiente/métodosRESUMEN
Understanding temporal and spatial trends in pregnancy and birth outcomes within an urban area is important for the monitoring of health indicators of a population. We conducted a retrospective cohort study of all births in the public hospital of Temuco, a medium-sized city in Southern Chile between 2009 and 2016 (n = 17,237). Information on adverse pregnancy and birth outcomes, as well as spatial and maternal characteristics (insurance type, employment, smoking, age, and overweight/obesity), was collected from medical charts. Home addresses were geocoded and assigned to neighborhood. We tested whether births and prevalence of adverse pregnancy outcomes changed over time, whether birth events were spatially clustered (Moran's I statistic), and whether neighborhood deprivation was correlated to outcomes (Spearman's rho). We observed decreases in eclampsia, hypertensive disorders of pregnancy, and small for gestational age, while gestational diabetes, preterm birth, and low birth weight increased over the study period (all p < 0.01 for trend), with little changes after adjusting for maternal characteristics. We observed neighborhood clusters for birth rate, preterm birth, and low birth weight. Neighborhood deprivation was negatively correlated with low birth weight and preterm birth, but not correlated with eclampsia, preeclampsia, hypertensive disorders of pregnancy, small for gestational age, gestational diabetes, nor stillbirth. Several encouraging downward trends and some increases in adverse pregnancy and birth outcomes, which, overall, were not explained by changes in maternal characteristics were observed. Identified clusters of higher adverse birth outcomes may be used to evaluate preventive health coverage in this setting.
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Diabetes Gestacional , Eclampsia , Hipertensión Inducida en el Embarazo , Nacimiento Prematuro , Embarazo , Femenino , Recién Nacido , Humanos , Nacimiento Prematuro/epidemiología , Estudios Retrospectivos , Chile/epidemiología , Resultado del Embarazo/epidemiología , Hospitales PúblicosRESUMEN
Implementation of regulatory standards has reduced exhaust emissions of particulate matter from road traffic substantially in the developed world. However, nonexhaust particle emissions arising from the wear of brakes, tires, and the road surface, together with the resuspension of road dust, are unregulated and exceed exhaust emissions in many jurisdictions. While knowledge of the sources of nonexhaust particles is fairly good, source-specific measurements of airborne concentrations are few, and studies of the toxicology and epidemiology do not give a clear picture of the health risk posed. This paper reviews the current state of knowledge, with a strong focus on health-related research, highlighting areas where further research is an essential prerequisite for developing focused policy responses to nonexhaust particles.
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Contaminantes Atmosféricos , Contaminantes Atmosféricos/análisis , Polvo/análisis , Monitoreo del Ambiente , Tamaño de la Partícula , Material Particulado/análisis , Emisiones de Vehículos/análisisRESUMEN
Atmospheric aerosols are important drivers of Arctic climate change through aerosol-cloud-climate interactions. However, large uncertainties remain on the sources and processes controlling particle numbers in both fine and coarse modes. Here, we applied a receptor model and an explainable machine learning technique to understand the sources and drivers of particle numbers from 10 nm to 20 µm in Svalbard. Nucleation, biogenic, secondary, anthropogenic, mineral dust, sea salt and blowing snow aerosols and their major environmental drivers were identified. Our results show that the monthly variations in particles are highly size/source dependent and regulated by meteorology. Secondary and nucleation aerosols are the largest contributors to potential cloud condensation nuclei (CCN, particle number with a diameter larger than 40 nm as a proxy) in the Arctic. Nonlinear responses to temperature were found for biogenic, local dust particles and potential CCN, highlighting the importance of melting sea ice and snow. These results indicate that the aerosol factors will respond to rapid Arctic warming differently and in a nonlinear fashion.
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Contaminantes Atmosféricos , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Polvo/análisis , Aprendizaje Automático , Tamaño de la Partícula , SvalbardRESUMEN
Road traffic constitutes a major source of air pollutants in urban Beijing, which are responsible for substantial premature mortality. A series of policies and regulations has led to appreciable traffic emission reductions in recent decades. To shed light on long-term (2014-2020) roadside air pollution and assess the efficacy of traffic control measures and their effects on public health, this study quantitatively evaluated changes in the concentrations of six key air pollutants (PM2.5, PM10, NO2, SO2, CO and O3) measured at 5 roadside and 12 urban background monitoring stations in Beijing. We found that the annual mean concentrations of these air pollutants were remarkably reduced by 47%-71% from 2014 to 2020, while the concurrent ozone concentration increased by 17.4%. In addition, we observed reductions in the roadside increments in PM2.5, NO2, SO2 and CO of 54.8%, 29.8%, 20.6%, and 59.1%, respectively, indicating the high effectiveness of new vehicle standard (China V and VI) implementation in Beijing. The premature deaths due to traffic emissions were estimated to be 8379 and 1908 cases in 2014 and 2020, respectively. The impact of NO2 from road traffic relative to PM2.5 on premature mortality was comparable to that of traffic-related PM2.5 emissions. The public health effect of SO2 originating from traffic was markedly lower than that of PM2.5. The results indicated that a reduction in traffic-related NO2 could likely yield the greatest benefits for public health.
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Contaminantes Atmosféricos , Contaminación del Aire , Contaminantes Atmosféricos/análisis , Contaminación del Aire/análisis , Beijing , Monitoreo del Ambiente/métodos , Dióxido de Nitrógeno , Material Particulado/análisis , Salud PúblicaRESUMEN
BACKGROUND: In February 2021, over one hundred scientists and policy experts participated in a web-based Workshop to discuss the ways that divergent evaluations of evidence and scientific uncertainties are used to delay timely protection of human health and the environment from exposures to hazardous agents. The Workshop arose from a previous workshop organized by the European Environment Agency (EEA) in 2008 and which also drew on case studies from the EEA reports on 'Late Lessons from Early Warnings' (2001, 2013). These reports documented dozens of hazardous agents including many chemicals, for which risk reduction measures were delayed for decades after scientists and others had issued early and later warnings about the harm likely to be caused by those agents. RESULTS: Workshop participants used recent case studies including Perfluorooctanoic acid (PFOA), Extremely Low Frequency - Electrical Magnetic Fields (ELF-EMF fields), glyphosate, and Bisphenol A (BPA) to explore myriad reasons for divergent outcomes of evaluations, which has led to delayed and inadequate protection of the public's health. Strategies to overcome these barriers must, therefore, at a minimum include approaches that 1) Make better use of existing data and information, 2) Ensure timeliness, 3) Increase transparency, consistency and minimize bias in evidence evaluations, and 4) Minimize the influence of financial conflicts of interest. CONCLUSION: The recommendations should enhance the production of "actionable evidence," that is, reliable evaluations of the scientific evidence to support timely actions to protect health and environments from exposures to hazardous agents. The recommendations are applicable to policy and regulatory settings at the local, state, federal and international levels.
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Informática Médica , Humanos , Incertidumbre , Educación , InternetRESUMEN
Objective: To estimate the point prevalence and likely ranges of pregnancy-induced hypertension, pre-eclampsia, gestational diabetes, low birth weight and preterm delivery in Latin America and the Caribbean, and evaluate the heterogeneity of the estimates. Methods: We conducted a systematic review and meta-analysis of observational studies reporting the prevalence of maternal and perinatal adverse outcomes in populations in Latin American and the Caribbean published between 2000 and 2019 in English, Spanish, or Portuguese. We searched PubMed, Embase, and LILACS. We estimated the point prevalence and evaluated overall heterogeneity and, in sub-group analyses, heterogeneity by study design and level of bias. Results: Of 1087 records retrieved, 50 articles were included in the review: two on hypertensive disorders of pregnancy, 14 on pre-eclampsia, six on gestational diabetes, nine on low birth weight and 19 on preterm birth. No meta-analysis for hypertensive disorders of pregnancy could be done because of the small number of studies. Point prevalence estimates and 95% confidence intervals (CIs) for pre-eclampsia, gestational diabetes, low birth weight, and preterm birth were: 6.6% (95% CI: 4.9%, 8.6%), 8.5% (95% CI: 3.9%, 14.7%), 8.5% (95% CI: 7.2%, 9.8%), and 10.0% (95% CI: 8.0%, 12.0%), respectively. We observed substantial heterogeneity overall and by study design. No major differences in estimates were observed by level of bias. Conclusions: The results of this study provide updated estimates of some of the most prevalent adverse pregnancy and perinatal outcomes in Latin America and the Caribbean. They highlight that important heterogeneity exists in prevalence estimates, which may reflect the diversity of populations in the region.
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This study aims to critically evaluate the source apportionment of fine particles by multiple receptor modelling approaches, including carbon mass balance modelling of filter-based radiocarbon (14C) data, Chemical Mass Balance (CMB) and Positive Matrix Factorization (PMF) analysis on filter-based chemical speciation data, and PMF analysis on Aerosol Mass Spectrometer (AMS-PMF) or Aerosol Chemical Speciation Monitor (ACSM-PMF) data. These data were collected as part of the APHH-Beijing (Atmospheric Pollution and Human Health in a Chinese Megacity) field observation campaigns from 10th November to 12th December in winter 2016 and from 22nd May to 24th June in summer 2017. 14C analysis revealed the predominant contribution of fossil fuel combustion to carbonaceous aerosols in winter compared with non-fossil fuel sources, which is supported by the results from other methods. An extended Gelencsér (EG) method incorporating 14C data, as well as the CMB and AMS/ACSM-PMF methods, generated a consistent source apportionment for fossil fuel related primary organic carbon. Coal combustion, traffic and biomass burning POC were comparable for CMB and AMS/ACSM-PMF. There are uncertainties in the EG method when estimating biomass burning and cooking OC. The POC from cooking estimated by different methods was poorly correlated, suggesting a large uncertainty when differentiating this source type. The PM2.5 source apportionment results varied between different methods. Through a comparison and correlation analysis of CMB, PMF and AMS/ACSM-PMF, the CMB method appears to give the most complete and representative source apportionment of Beijing aerosols. Based upon the CMB results, fine aerosols in Beijing were mainly secondary inorganic ion formation, secondary organic aerosol formation, primary coal combustion and from biomass burning emissions.
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Contaminantes Atmosféricos , Material Particulado , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Beijing , Monitoreo del Ambiente , Humanos , Material Particulado/análisisRESUMEN
Wintertime urban air pollution in many global megacities is characterised by episodic rapid increase in particulate matter concentrations associated with elevated relative humidity - so-called haze episodes, which have become characteristic of cities such as Beijing. Atmospheric chemistry within haze combines gas- and condensed-phase chemical processes, leading to the growth in secondary species such as sulphate aerosols. Here, we integrate observations of reactive gas phase species (HONO, OH, NOx) and time-resolved aerosol composition, to explore observational constraints on the mechanisms responsible for sulphate growth during the onset of haze events. We show that HONO abundance is dominated by established fast gas-phase photochemistry, but the consideration of the additional formation potentially associated with condensed-phase oxidation of S species by aqueous NO2 leading to NO2- production and hence HONO release, improves agreement between observed and calculated gas-phase HONO levels. This conclusion is highly dependent upon aerosol pH, ionic strength and particularly the parameterisation employed for S(iv) oxidation kinetics, for which an upper limit is derived.
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We present shipborne measurements of size-resolved concentrations of aerosol components across ocean waters next to the Antarctic Peninsula, South Orkney Islands, and South Georgia Island, evidencing aerosol features associated with distinct eco-regions. Nonmethanesulfonic acid Water-Soluble Organic Matter (WSOM) represented 6-8% and 11-22% of the aerosol PM1 mass originated in open ocean (OO) and sea ice (SI) regions, respectively. Other major components included sea salt (86-88% OO, 24-27% SI), non sea salt sulfate (3-4% OO, 35-40% SI), and MSA (1-2% OO, 11-12% SI). The chemical composition of WSOM encompasses secondary organic components with diverse behaviors: while alkylamine concentrations were higher in SI air masses, oxalic acid showed higher concentrations in the open ocean air. Our online single-particle mass spectrometry data exclude a widespread source from sea bird colonies, while the secondary production of oxalic acid and sulfur-containing organic species via cloud processing is suggested. We claim that the potential impact of the sympagic planktonic ecosystem on aerosol composition has been overlooked in past studies, and multiple eco-regions act as distinct aerosol sources around Antarctica.
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Contaminantes Atmosféricos , Ecosistema , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Regiones Antárticas , Monitoreo del Ambiente , SulfatosRESUMEN
Airborne particulate matter (PM) is a pollutant of concern not only because of its adverse effects on human health but because of its ability to reduce visibility and soil buildings and materials. It can be regarded as a suite of pollutants since PM covers a very wide range of particle sizes and also has a diverse chemical composition. Historically, much of the PM arose from coal burning and was measured as black smoke. However, in the second half of the twentieth century in developed countries, there was a reduction in black smoke emissions from coal burning and PM steadily became dominated by carbonaceous particles from road traffic exhaust and the secondary pollutants, ammonium salts and secondary organic carbon. This is exemplified by the composition of fine particles (referred to as PM2.5) as measured in London, Delhi and Beijing. Steadily, as control strategies have addressed the more tractable sources of emissions, so sources previously regarded as unconventional have emerged and have been seen to make a significant contribution to airborne PM concentrations. Among these are non-exhaust particles from road traffic, cooking aerosol and wood smoke. The particle size distribution of airborne PM is hugely diverse, ranging from newly formed particles of a few nanometres in diameter through to particles of tens of micrometres in diameter. There has been a great deal of interest in ultrafine (nano) particles because of suspicions of enhanced toxicity, and as traffic emissions decrease as a source, so regional nucleation processes have become much bigger relative contributors to particle number, but not mass. This article is part of a discussion meeting issue 'Air quality, past present and future'.
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Particulate and vapor phase emissions in the diluted exhaust of a light-duty diesel engine designed for Euro 5 application have been sampled. The engine was operated in three modes, and samples were collected from the exhaust without aftertreatment but also with aftertreatment by an exhaust oxidation catalyst and particle filter. The samples were analyzed by two-dimensional gas chromatography with time-of-flight mass spectral detection. The results show overall removal efficiencies for the organic compound mass by the combination of oxidation catalyst and particle filter of 50, 56, and 74% for the high-speed/high-load, low-speed/low-load, and high-speed/low-load conditions respectively. The results are clearly indicative of substantial repartitioning of the particulate and vapor components within the abatement devices and show an apparently reduced efficiency for the removal of high-molecular-weight alkanes under high-speed/high-load conditions relative to lower-molecular-weight compounds, although this may be due to alkane formation by thermocracking of other species. A notable feature is the presence of oxygenated compounds in the emissions, which are not present in the fuel. These are increased under high-speed/high-load conditions, and the results suggest the formation in the aftertreatment devices as well as in the combustion process.
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Polvo , Emisiones de Vehículos , Catálisis , Gases , Oxidación-ReducciónRESUMEN
In the austral spring, biomass fires affect a vast area of South America each year. We combined in situ ozone (O3) data, measured in the states of São Paulo and Paraná, Brazil, in the period 2014-2017, with aerosol optical depth, co-pollutants (NOx, PM2.5 and PM10) and air backtrajectories to identify sources, transport and geographical patterns in the air pollution data. We applied cluster analysis to hourly O3 data and split the investigation area of approximately 290,000â¯km2 into five groups with similar features in terms of diurnal, weekly, monthly and seasonal O3 concentrations. All groups presented a peak in September and October, associated with the fire activities and enhanced photochemistry. The highest mean O3 concentrations were measured inland whilst, besides having lower concentrations, the coastal group was also associated with the smallest diurnal and seasonal variations. The latter was attributed to lower photochemical activity due to frequently occurring overcast weather situation. The mean annual regional contribution of O3 over the area was 61⯵g/m3, with large seasonal and intersite variabilities (from 35 to 84⯵g/m3). The long-range transport of smoke contributed with between 23 and 41% of the total O3 during the pollution events. A pollution outbreak in September 2015 caused many-fold increases in O3, PM2.5 and PM10 across the investigation area, which exceeded the World Health Organisation recommendations. We show that the regional transport of particulates and gas due to biomass burning overlays the local emissions in already highly polluted cities. Such an effect can outweigh local measures to curb anthropogenic air pollution in cities.
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Contaminantes Atmosféricos , Contaminación del Aire , Meteorología , Ozono , Biomasa , Brasil , Ciudades , Monitoreo del Ambiente , Estaciones del AñoRESUMEN
Machine learning techniques (MLTs) offer great power in analyzing complex data sets and have not previously been applied to non-occupational pollutant exposure. MLT models that can predict personal exposure to benzene have been developed and compared with a standard model using a linear regression approach (GLM). The models were tested against independent data sets obtained from three personal exposure measurement campaigns. A correlation-based feature subset (CFS) selection algorithm identified a reduced attribute set, with common attributes grouped under the use of paints in homes, upholstery materials, space heating, and environmental tobacco smoke as the attributes suitable to predict the personal exposure to benzene. Personal exposure was categorized as low, medium, and high, and for big data sets, both the GLM and MLTs show high variability in performance to correctly classify greater than 90 percentile concentrations, but the MLT models have a higher score when accounting for divergence of incorrectly classified cases. Overall, the MLTs perform at least as well as the GLM and avoid the need to input microenvironment concentrations.
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Benceno , Contaminación por Humo de Tabaco , Monitoreo del Ambiente , Modelos Lineales , Aprendizaje AutomáticoRESUMEN
Although GC×GC-ToF-MS allows the separation of thousands of peaks, many of these peaks are not positively identified owing to the lack of mass spectral library data and/or standard materials, leading to a substantial amount of information being inaccessible. The fragmentation patterns of molecules in mass spectrometers using electron impact ionization at 70 eV can be useful for molecule identification, provided a match is available in a published EI MS library, but are indistinguishable for many isomeric organic compounds (for example, linear and branched alkanes). Lower ionization energies have been exploited leading to organic compounds being ionized with lower excess internal energy and less fragmentation, retaining the molecular ion and maximizing its relative signal. This has enabled the identification of a large number of isomeric organic compounds, both aliphatic and aromatic, between C12-C36, in the previously unresolved complex mixture (UCM) of two motor oil samples. This technique also demonstrates problems associated with separation of coeluting isomers, particularly for the n-alkanes, which are routinely measured by 1D GC/MS and may be overestimated, due to coelution. As a consequence retention times in 2 dimensions and mass spectra at variable ionization energies are shown to give unparalleled power to identify specific isomers.